Universal features in the lifetime distribution of clusters in hydrogen-bonding liquids

Abstract

Hydrogen bonding liquids, typically water and alcohols, are known to form labile structures (network, chains, etc...), hence the lifetime of such structures is an important microscopic parameter, which can be...

Lifetime Distribution of Clusters in Binary Mixtures Involving Hydrogen Bonding Liquids

“…The second striking feature is that there is a very small concentration dependance of the lifetimes L(t). As explained in 12 , but also in the introductory part to this section, the various curves shown in each panel show 2 typical features. A series of high peaks dominate the figures, whose maximum is seen to move to larger times with increasing r c values, as well as decreasing in amplitude.…”

“…What we observe is that these 2 secondary and tertiary maximum are now nearly insensitive to r c , in contrast to the first maximum of the inset, suggesting that the typical lifetimes corresponding to these maximum, do not depend on r c . In 12 , we have attributed the first maxima to oxygen dimer lifetimes, while the secondary and tertiary r c independent maximum where attributed respectively to larger clusters and to their shape dependence. We have provided several evidences to support this interpretation.…”

“…Fig. 1 is an introductory reminder of the features reported in 12 , which should serve as a guidance to study the various mixtures studied herein. Typical points are depicted in specific colors corresponding to the curves shown in the left panel.…”

“…This secondary life time is quite short, about τ 2 ≈ 0.02ps. The tertiary peak has been interpreted in 12 as a related to the very specific shape of the clusters, such as globules, chains, branched, loops, etc..., which are seen to appear very often in associated liquids such as water and alcohols, for example. These particularly shaped clusters live longer lifetimes, and the tertiary life time is approximately τ 3 ≈ 0.05ps.…”

“…Interestingly, only the correlations has been the focus of previous studies [8][9][10][11] . In a recent work 12 , based on a classical description of Hbonding through Coulomb charge association, we have examined the lifetime L(t) of the Hbond, which is related to the average of h i j (t), for several Hbonding molecules, such as water, alcohols and amines, defined as follows:…”